151. Density functional theory study on the interaction of H2 and CO with Fe2O3 based on hydrogen-based shaft furnace process.
- Author
-
Liu, Xicai, Tang, Jue, Chu, Mansheng, Zhao, Zichuan, Feng, Jinge, Liu, Jie, and Tang, Zhidong
- Subjects
- *
DIRECT-fired heaters , *DENSITY functional theory , *FERRIC oxide , *IRON clusters , *ACTIVATION energy - Abstract
The adsorption behaviors, reaction pathways and coupling mechanism of α-Fe 2 O 3 (0001) surface with the H 2 molecules and CO molecules in hydrogen-based shaft furnace were investigated at the atomic level based on the density functional theory. The results showed that the most stable adsorption configuration of H 2 molecule has an adsorption energy of −1.65 eV, whereas CO molecule is −2.10 eV. The most stable adsorption sites are both O atom, but the adsorption of CO molecule is more stable compared to H 2 molecule. The energy barrier of H 2 molecule is 0.64 eV and 0.76 eV of energy need to be absorbed after generating one free H 2 O molecule. While CO molecule reacts with an energy barrier of 1.40 eV and 0.09 eV of energy has to be released after generating one free CO 2 molecule. The reaction of H 2 molecules with Fe 2 O 3 is kinetically dominant but thermodynamically adverse. Increasing the temperature is detrimental to the adsorption of gas molecules but favors the reduction reaction, and can compensate for the thermodynamic disadvantage of adsorption and reaction for H 2 molecules. The adsorption energy per H 2 molecule is −1.51 eV and that of per CO molecule is −1.03 eV. The adsorption energy of −2.67 eV for the co-adsorption of one H 2 molecule and one CO molecule is less than the linear sum of adsorption energies when they adsorb separately, suggesting a synergistic mechanism for the interaction of H 2 and CO with Fe 2 O 3. This work can provide theoretical guidance for hydrogen-rich or even pure hydrogen reduction in hydrogen-based shaft furnace. • The adsorption of H 2 is unstable compared to CO and the most stable sites are O. • The reaction energy barrier of H 2 is lower than CO, which is kinetically dominant. • Increasing the temperature can compensate for the thermodynamic disadvantage of H 2. • A synergistic mechanism for the interaction of H 2 and CO with Fe 2 O 3. [ABSTRACT FROM AUTHOR]
- Published
- 2024
- Full Text
- View/download PDF